Publications
Revisiting the WIPP humic colloid model for tetravalent actinides
Humic complexation has the potential to increase actinide mobility and hamper waste isolation in geologic nuclear waste repositories. This study shows that humic complexation of tetravalent actinides (Th(IV), U(IV), Np(IV), and Pu(IV)) has been overestimated in past performance assessments of the Waste Isolation Pilot Plant (WIPP). Major reductions are needed for PHUMSIM and PHUMCIM, the equilibrium concentration ratios of humic-bound aqueous actinide to non-colloidal aqueous actinide. These coefficients are currently set at a value of 6.3 based on Th(IV) measurements in particle size fractions of seawater. Actual humic partitioning is expected to be significantly lower in WIPP brines primarily because pH is higher (∼9) and concentrations of competing cations (e.g., Mg2+) are higher. In this work, data from recent studies of Th(IV)-humic, U(IV)-humic, and Ca2+-humic complexation are used to simulate competitive humic complexation under WIPP repository conditions and to estimate new An(IV) PHUMSIM and PHUMCIM values. The new lower coefficients reduce the humic-bound An(IV) concentrations by more than 99%, causing a reduction in total mobile An(IV) concentrations by 85% to 86%, assuming no other type of An(IV) colloid (i.e., intrinsic, microbial, and mineral fragment colloids) is present in significant concentrations.